Comprehensive simulations of stimuli-responsive soft porous materials

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Molecular switching units embedded in soft porous materials such as Metal-Organic Frameworks (MOFs) and Covalent Organic Frameworks (COFs) offer a versatile platform for the development of stimuli-responsive materials. Using the framework structure as a scaffold, the arrangement and orientation of the responsive molecular building units can, in principle, be precisely modulated and thus tailored for various applications such as molecular storage or catalysis. However, despite the advances in the development of these stimuli-responsive soft porous materials, the understanding of fundamental aspects with respect to the structural and dynamic properties is still limited. By developing and applying a force field library to accurately and efficiently describe the molecular switching units, the goal of this research project is to reveal coupled and cooperative phenomena based on the embedded responsive molecular units. Different classes of molecular switches, including mechanically interlocked species, immobilized in systematically modified soft porous materials (e.g., network topology, pore dimension) will be studied. In this context, parametrization algorithms will be developed enabling to parametrize in detail the switching pathway of the responsive molecular species. Based on this, not only the structural properties of the functionalized frameworks but rather the dynamic interplay of the responsive molecular units with each other and their interactions with guest molecules will be investigated by atomistic simulations. To decipher the impact of nano-confinement induced by the soft porous materials, simulations of molecular switches embedded in a solvation environment will be performed, and the results will be compared and quantitatively evaluated. These comprehensive studies are expected to provide a fundamental understanding of the spatial and temporal control of molecular phenomena in stimuli-responsive porous materials.